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Composites: Part A 30 (1999) 667682

Optimisation of a GMT-based cold pressing technique for low cost textile


reinforced thermoplastic composites
Sofie Baeten*, Ignaas Verpoest
Department of Metallurgy and Materials Engineering, KULeuven, de Croylaan 2, B-3001 Leuven, Belgium
Received 15 February 1998; received in revised form 15 July 1998; accepted 5 August 1998

Abstract
Much potential and interest exists for the fast processing of lightweight, inexpensive composite preforms in automotive and other transport
applications. As a thermoplastic matrix is more suitable for mass production with short cycle times, a novel cost-effective glass fibre
reinforced thermoplastic textile preform is developed. Weft-inserted warp knitting is used to produce this textile preform containing both
the reinforcing fibres and the thermoplastic matrix material as split-film ribbons. The aim of the work is to establish a useful processing
technique and to control those parameters which lead to the production of good quality composite parts. The current study is specifically
directed at determining the feasibility of the GMT-based cold pressing technique for the manufacturing of this new type of thermoplastic
composite. An experimental design method is used to develop a statistical model which gives response surfaces of the effects of the
processing parameters on the mechanical performance of the final composite part. Processing variables are ranked in order of importance
to determine the optimal processing window. An economical comparison with the use of long fibre reinforced GMT mats proves the costefficiency of this new continuous reinforced thermoplastic composite. 1999 Elsevier Science Ltd. All rights reserved.
Keywords: Thermoplastic

1. Introduction
Enhanced safety standards and extended luxury demands
have tremendously increased the weight of vehicles. Fibre
reinforced composite materials offer, besides Al and Mg, a
significant lightweight potential in structural body parts of
vehicles [1]. Due to some severe disadvantages of thermoset
composites, such as long production times, limited recyclability, constrained storage time as well as storage requirements, interest in thermoplastic composites has developed
recently [2]. Despite a promising cost decrease when using a
thermoplastic matrix, the raw material price level is as yet
far from that of competing lightweight metals. A growth in
the use of thermoplastic composites currently depends on
further reduction of the manufacturing cost and optimisation
of the part performance. A decrease in the fabrication cost of
thermoplastic composite parts can be obtained if the separate impregnation step is eliminated, by means of a dry
impregnation [1]. Amongst other techniques such as
powder impregnation, melt and solvent impregnation, film
stacking and fibre co-mingling [8,17,18], the use of textile
preforms has recently been studied. Moreover, the difficult
* Corresponding author. Tel.: 32-16-32-11-95; fax: 32-16-32-19-90.
E-mail address: sofie.baeten@mtm.kuleuven.ac.be (S. Baeten)

impregnation of the reinforcing fibre bundles due to the high


matrix viscosity and low shear flow rates can be overcome
by the use of several types of combined yarns, where the
reinforcing fibres are intensely mixed with the matrix prior
to composite processing [4]. To further reduce the mass
transfer of the matrix during processing compared to film
stacking, the development of a new inexpensive thermoplastic textile preform using existing textile processing
techniques, is the first goal of the current study [5].
In all material developments for mass applications, the
processability in an industrial environment, is an important
issue. The three stage process cycle of thermoplastic
composites consists of preheating the matrix polymer
above its melting point, followed by a compaction to wetout the reinforcement and to give the shape to the part, and a
final cooling down [4,9]. The matrix must be heated sufficiently above its melting point to reduce the viscosity for
full fibre impregnation. While overheating will degrade the
polymer, the preheating stage is critical and can be mainly
achieved in two ways.
The in-mould matched-die hot moulding, where a loose
stack of dry preform layers is heated, pressed and cooled
down in the mould, involves high heating energy flow to
and from the forming equipment, resulting in long cycle

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S. Baeten, I. Verpoest / Composites: Part A 30 (1999) 667682

times and high operating costs. This hot pressing process


is hence far too expensive for industrial use.
During an alternative cold pressing method, the fabric is
preheated separately in an external oven prior to transfer
to the forming equipment, which is at a temperature
below the melt temperature of the thermoplastic matrix.
This technique is well established in GMT (Glass Mat
reinforced Thermoplastic) processing and eliminates the
cycling of the mould temperature, avoiding large cycle
times. However, in classical GMT-processes, preimpregnated materials are used, and the GMT-processing is
mainly used to shape the part.
Hence, an additional goal of the present work is the development of an adequate fast manufacturing technique to
produce split-warpknit composites in a cost-effective
manner. The feasibility of the GMT-based cold pressing
technique for this type of material in non-preimpregnated
form, is evaluated.
2. Split-warpknit textile preform
Special glass sizings and a low viscosity PP matrix material are developed to ensure a good wetting out of the glass
fibre reinforcement and an easy, thus fast impregnation.
The PP recipe Shell XS 6500 was stabilised and modified
with 2 wt% Polybond 3150 to achieve a quick wetting of the
glass fibres by the low-viscosity matrix (MFI 230/2.16 [g/
10 min] 36). The material properties are characterised by
GPC, DCS and FTIR. No hint of degradation during heating
at the proposed maximum thermal (240C) and time
(10 min) conditions could be detected. The viscosity
shear behaviour is determined by a plate/plate arrangement
in the temperature region between 200 and 260C and a
frequency sweep of 0.1100 rad/s. By means of a superposition principle of temperature and time, a master curve
was determined for 200C. The master curve shows exact
superposition of all measured curves. It can be concluded
that in the tested temperature region no morphological
changes occur in the melt. The temperature dependency of
the viscosity is calculated by the Arrhenius Law and an
energy of activation of 39.1 kJ/mol is obtained.
Glasseiden GmbH Oschatz produced the filament yarns
(EC 14 300 tex 35/8), appropriate for warp knitting, based
on the sizing investigated by IPF (Institut fur Polymerforschung, Dresden). The commercial aminosilane A1100
(OSi Specialties) is used as the silane coupling agent. The
film former combination is varied to approach the best
conditions for knitting (high mechanical loading) and on
the other hand to obtain open rovings to ensure a good
wetting behaviour of the bundles. It is known that PPdispersions are good compatible film formers in PPmatrices. Two commercial PP-dispersions, Protolube 3974
and Icopol OC, are used. These dispersions are blended with
the polyurethane(PUR)-dispersion Neoxil 9851, which is
necessary for the processing.

Split-film is a special term for a continuous thermoplastic film that has been cut lengthwise into tapes of
small cross section. The resultant yarn is much less
expensive than conventional (i.e. spun) fibres, but is
nevertheless well-suited to classical textile operations.
Warp knitting of split-film only, has been known for a
long time as a favourable technique to produce low-cost
net-type textile structures in large volumes. Warp knits
also exhibit a great drapability. For this reason it was
intended to combine warp knitting of split-films with
weft-inserted reinforcement fibres to obtain a non-crimp
fabric. Hence, weft-inserted multi-axial warp knitting is
chosen for its low production cost to produce the SPLITWARPKNIT thermoplastic textile preform containing
both non-crimp reinforcing fibres and thermoplastic
matrix ribbons (Fig. 1). It allows for non-impaled knitting where the loop formation is achieved without needling through the fabric and a degradation of the
mechanical properties due to a premature damage of
the reinforcing fibre bundles is avoided. Instead, the
weft-inserted yarns are placed parallel to the needle
row in a one by one manner. The split-films are either
used as warp knitting yarn (see Fig. 1: co-knitted structure)
where the glass fibres are inserted along the weft and warp
direction (bi-axial textile) or they are inserted in the straight
yarns along with the reinforcement rovings. The loops,
hence, exclusively consist of a binding yarn (PET yarn)
(Fig. 1: hybrid mono-axial structure).
The merit of this new split-warpknit textile is that a
composite part can eventually be made in only one step
directly from the dry textile preform, without the further
addition of matrix material. No intermediate production
steps, which prolong the cycle time, should be necessary.
The main issue during the production of thermoplastic
composites is, however, the impregnation of the reinforcing
fibres by the highly viscous thermoplastic matrix. During
impregnation, the polymer matrix has to flow through
closely packed fibre bundles and wet-out the individual
fibres, while high temperature and pressure is applied. The
impregnation time is controlled by the velocity and the ease
of flow of the thermoplastic matrix to guarantee a good
adhesion between the fibre and the matrix. Different
preforming techniques have indeed been developed to intermingle the fibre and the matrix in a dry textile structure to
reduce the flow distance and decrease the impregnation
time. Co-mingled yarns where glass fibres and thermoplastic polymer yarns are brought together in one bundle (cf.
Twintex yarn from Vetrotex) are nowadays of increasing
interest. The new split-warpknit structure comprising the
reinforcing glass fibres and the thermoplastic PP split-film
ribbons in one hybrid yarn, held together with a nonmeltable PET binding yarn (see Fig. 1) also results in an
improved impregnation homogeneity and good mechanical
properties. The split-warpknit textile is hence competitive
with other commercial materials already available on
the market [10,19].

S. Baeten, I. Verpoest / Composites: Part A 30 (1999) 667682

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Fig. 1. Mono-axial hybrid split-warpknit thermoplastic textile preform (weft-inserted). Bi-axial co-knitted split-warpknit thermoplastic textile preform (weftand warp-inserted).

The advantages of this class of thermoplastic split-warpknit textile preforms can be summarised [6,7]:
low production cost of the textile structure because thermoplastic ribbons are used;
preform shows a good drapability: complex parts can be
made in a one step process from dry textile to final
composite part;
increased mechanical properties of the composite due to
the non-crimp textile structure;
one textile structure is composed of different layers, with
different orientations of the reinforcing fibres. It is hence
a multi-layer, multi-axial (weft and warp insertion of
reinforcing glass fibre bundles) preform which enhances
the part cost efficiency;
short cycle processing time is possible: this thermoplastic
textile preform is processable with the GMT-based cold
pressing technique, allowing for a fast production using
commercially available moulding equipment;
as the hybrid yarn structure determines the homogeneity
of the distribution of the reinforcing fibres in the polymer
matrix and thus the mechanical performance, a good
composite part can be made.

3. GMT cold pressing technique


Given the apparent potential for the application of thermoplastic fabric composites in high volume manufacturing,
the conflicting demands of process cycle time and laminate
quality require to be resolved.
The main objective of research into processing

thermoplastic composites is to determine the optimal


processing window. This is mainly defined as the
narrow region of temperatures between a lower bound
below which unsatisfactory impregnation of the fibres
by the highly viscous thermoplastic matrix occurs and
an upper bound beyond which matrix degradation
through oxidation occurs due to exposure to excessive
temperatures.
As the duration of the heating and the cooling phase is the
bottleneck when optimising the cycle time in matched-die
compression moulding, the idea arose to use and modify a
GMT-like manufacturing technique with an external
preheating phase and a cold mould pressing (Fig. 2), so
that it can be used for the non-preimpregnated split-warpknit material.
The first goal of the study was to investigate whether it is
possible to use an external preheating phase and a cold
pressing process for the one step production of the dry thermoplastic split-warpknit preform into a final composite part.
Secondly, a systematic optimisation of the different process
parameters is performed using an experimental design
method.
Considering the two stage process of external heating
under slight pressure, transferring the molten material to
the cold mould and consolidating under pressure, the
following process parameters are of importance:
Preheating phase
preheating method
preheating temperature
preheating time

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S. Baeten, I. Verpoest / Composites: Part A 30 (1999) 667682

Fig. 2. Overview of the GMT-based production technique: one step process from dry textile preform to final composite part.

Cold pressing
mould temperature
consolidating pressure
holding time at pressure

4. Results and discussion


4.1. Applicability of the GMT cold pressing method
4.1.1. Feasibility of the external preheating phase:
preheating method
During the manufacturing of thermoplastic films, polymer chains get a high degree of orientation due to stretching.
When heated without applying any external pressure, the
highly oriented molecular chains in the stretched film
ribbons return to their more natural state of random coil
orientation, resulting in a considerable shrinkage of the thermoplastic film ribbons. Due to this significant shrinkage of
the preform, it is necessary to support the dry textile
throughout the heating phase to prevent an uncontrolled
shrinkage of the film ribbons causing waviness of the fibres.
As a consequence, the mechanical performance of the final
composite part decreases. An extensive analysis of the
shrinkage behaviour pointed out that a minimum external
pressure is needed to create sufficient friction which can
avoid waviness of the non-crimp reinforcing fibres [11].
Typical preheating methods in the GMT technique
include infrared (IR), conduction and convection heating
[3].
IR heating has been proven to be a good choice when
heating thin, well-compacted sheets. Because IR heating
mostly occurs at the surface and must be conducted away

from the surface to prevent overheating, it is not a suitable


method for heating a loosely stacked pile of textile layers.
Moreover, no external support is given to avoid the shrinkage of the thermoplastic ribbons in the split-warpknit.
Convection heating also causes oxidation and degradation unless it is performed in an inert atmosphere.
During conductive heating between two press plates,
oxidation and degradation are reduced because the material
is shielded from the atmosphere. The textile layers, heated
above the melt temperature of the polymer matrix, are flexible, easily distorted and they additionally tend to stick to
the contact surface of the hot platens during conductive
heating. This makes handling rather difficult.
After evaluation of the different heating systems, only
conductive heating of the pile of dry textile layers between
the platens of a hot press at very low pressure (4 bar) is
fast enough to prevent the matrix from sinking out due to
gravity [12]. The low pressure conveys the air out of the
loose stack of textiles and increases the heating speed.
However, the stickiness of the molten polypropylene
becomes a problem during heating and transportation from
the preheating device to the mould. This problem could be
solved by placing the stack of textile layers between two
Teflon sheets. After transferring the molten textile layers
between two flexible teflon carriers, a flat laminate is subsequently pressed in a cold mould. The use of this Teflon film
also results in a good surface quality of the pressed laminates. Moreover, the Teflon foil can be re-used during
further trials.
Though conductive heating seems to be the faster
method, it is not convenient for use in a continuous production process [2] and it is a rather expensive technique. IR
heating could be an alternative, fast and convenient heating
method if the uncontrolled shrinkage of the PP ribbons can

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671

Fig. 3. Influence of the holding time on the tensile modulus and strength of cross ply split-warpknit laminates of the bi-axial co-knitted split-warpknit.

be eliminated. One possibility is to include, prior to the IR


heating, an additional continuous pre-compaction phase at
low pressure and intermediate temperature to relax the internal stresses in the stretched ribbons and hence avoid the
shrinkage of the split-films. The results of this ongoing
study of an additional pre-compaction phase will be
reported elsewhere.
4.1.2. Feasibility of short cycle cold pressing
It is essential to investigate whether it is possible to use a
short cycle cold pressing method instead of the matched-die
moulding technique. Any alteration of the ideal, uneconomical classical production process has an influence on the
impregnation and distribution of the fibres throughout the
composite. While in the in-mould heating process the
impregnation time is a programmable parameter, this is no
longer the case for the GMT-based production process.
To study the influence of the different cold pressing
parameters, the tensile modulus and strength of cross ply
laminates of the co-knitted bi-axial split-warpknit (see Fig.
1) were determined with an Instron 4045, using hydraulic
clamps. The tensile modulus of a test specimen is the average value of its tangent moduli calculated between 0.48%
and 0.52% strain. Each result is the average value of six
different samples tested, where the reproducibility within
one parameter array is very high (within 5%).
Because the shear properties are more matrix and interface controlled than the tensile properties (0, parallel to and
90, perpendicular to the fibres) and hence the influence of
the processing conditions on the impregnation quality and
wetting out of the fibres will be more pronounced, 45
tensile tests on the bi-axial co-knitted split-warpknit were

also carried out to determine the in-plane shear modulus


(ASTM 3518-91)
Gxy

E45
21 nxy

where Gxy is the in-plane shear modulus (in GPa), E45 is the
tensile modulus achieved during a tensile test of a ^45
laminate (in GPa) and nxy is the Poisson coefficient.
No shear strength is determined due to a plastic yielding
of the thermoplastic PP matrix. In the ^45 tensile test, both
the longitudinal and transversal strains have to be measured.
The derivation of the formula for a 45 tensile test is
presented in Ref. [20].
During a first feasibility study, the relative importance of
the different cold pressing parameters (temperaturepressuretime) on the tensile and shear behaviour of cross ply
laminates of the bi-axial co-knitted split-warpknit textile is
hence determined. Also the influence of the preheating
temperature was further considered [12].
It was proved that the mould pressure does not affect the
tensile modulus and strength of the cross ply [0,90] splitwarpknit composite laminate. Probably there will be a minimum pressure needed to make the highly viscous thermoplastic matrix flow through the closely packed glass fibres
and to guarantee a sufficient wet-out of the glass fibre
bundles by the PP. This minimum could, unfortunately,
not be determined with the actual press, which has a minimum pressure of 0.8 bar.
The influence of the holding time at high pressure on the
tensile properties of the cross ply [0,90] is negligible once a
certain minimum time (^30 s) is reached (Fig. 3). Because

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S. Baeten, I. Verpoest / Composites: Part A 30 (1999) 667682

Fig. 4. Temperature profile of the bi-axial split-warpknit textile, when placed in the mould (laminate thickness 2.53 mm).

of the enormous mass difference between the composite and


the mould and because of the high thermal diffusivity of
metals, the composite plate cools down very fast once the
mould is closed. The temperature was continuously
measured in the mid-plane of the laminate (thickness of
around 2.53 mm), while closing the mould (Fig. 4). The
closing time of the mould was around 15 s with a temperature drop of only 16C. When the mould is effectively closed
and pressure is applied, the temperature of the composite
plate drops 100C in only 20 s. Because the cooling of the
material to the mould temperature is very fast and the
selected mould temperatures are far below the melt
temperature of PP, further impregnation and wetting out
of the fibres is not likely to occur because the matrix

becomes too viscous. It is therefore obvious that the


mould temperature does not effect the mechanical properties of the composite.
The only processing parameter of major importance for
the tensile behaviour is the preheating temperature, the
temperature to which the preform is externally heated in
an oven before it is formed in a cold mould (Fig. 5). This
temperature greatly influences the viscosity of the thermoplastic matrix and hence the ease of wetting out and flow
through the closely packed fibres. This is even more
pronounced when studying the shear modulus in ^45
tensile tests (Fig. 6). The pressure and the mould temperature influence the shear modulus to a much lower extent.
While the GMT cold pressing technique is feasible for

Fig. 5. Influence of the preheating temperature on the tensile modulus and strength of a symmetric cross ply [0,90] laminate of the bi-axial split-warpknit
textile.

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Fig. 6. The influence of the preheating temperature on the 45 tensile modulus E45 and shear modulus Gxy of a cross ply laminate of the bi-axial split-warpknit,
tested under 45.

split-warpknits, it yields somewhat lower composite


mechanical properties compared to the matched-die hot
pressing process. It is, nevertheless, a very worthwhile
consideration in low-cost applications, especially because
existing equipment can be used. Further optimisation of
the GMT cold pressing technique for the split-warpknit
material is hence meaningful.
4.2. Experimental design method: optimal processing
window

variation in preheating temperature and time, mould


pressure and temperature, and holding time. The Taguchi
study is performed during the screening and the first optimisation phase.
During the EVOP (evolutionary operation) method the
new experimental set-up is designed in the direction of the
steepest ascent of the former optimisation step. The EVOP
method is applied during the second optimisation steps. An
overview of the strategy is given in Fig. 7.
4.2.2. Optimisation procedure

The GMT cold pressing method is further optimised


using an experimental design method to reach the optimal
processing window in an efficient way [4,13]. In a designed
experiment, the series of tests are determined beforehand
where planned changes are made to the production parameter settings to observe and identify changes in the output
properties [1416].
4.2.1. Experimental design method
In an experimental design, a test matrix is constructed
with the important process parameters and interactions set
at a high and low value. The range between the low and high
level is taken as broad as possible to surely hold the optimal
parameter settings. Two different experimental design techniques are used during this study.
A well-known Taguchi study is performed to investigate
the effects of processing parameters on the flexural behaviour of split-warpknit laminates [14]. The study includes

4.2.2.1. Screening. During the screening phase, the different processing parameters were set at two levels in an L16
array (fractional factorial design), performing 16 experiments (see Table 1). This set-up even allows for the evaluation of the significance of first-order interactions between
the different processing parameters:
pressure and holding time
pressure and mould temperature
holding time and mould temperature
preheating time and holding time
preheating time and mould temperature
preheating temperature and mould temperature
preheating time and preheating temperature
The optimisation study is, however, performed for the
mono-axial GF/PP split-warpknit with a PET binding yarn
(see Fig. 1), because this hybrid structure shows superior

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S. Baeten, I. Verpoest / Composites: Part A 30 (1999) 667682

Fig. 7. Optimisation strategy for the GMT cold pressing technique.

properties to the co-knitted textile because of the smaller


flow distance for the thermoplastic matrix to impregnate the
fibre bundles. Cross ply laminates (90,0,90)2s were tested in
three-point bending. Flexural tests with the fibres of the
outer top and bottom layer oriented in the 90 direction
were performed to also include interphase effects and to
get more information about the impregnation quality due
to the appearance of normal (outer 90 layers) and shear
stresses (middle 0 layers) which allows a good characterisation of the material concerning the impregnation quality.
A statistically based model is derived to predict the flexural
properties of the split-warpknit composites at any processing level between the lower and upper limit of the parameter settings. The magnitude of the parameter effects is
investigated by an analysis of means, ANOM, using a
response table, while the significance of the effects is

determined by performing an analysis of variance,


ANOVA method [14].
The plot in Fig. 8 shows the effect of the main parameters
on the flexural modulus. A similar behaviour can be seen for
the bending strength (Fig. 9). When ranking the processing
parameters in order of importance, it is clearly seen that the
preheating time and the mould pressure have the largest
effect on the flexural stiffness and strength of the composite
(steepest slope in the response curve). The effect of the
relevant first-order interactions is summarized in Fig. 10,
where there is no interaction present for two perfectly parallel curves. It is already obvious that there is a significant
interaction between the preheating time and the holding
time (Fig. 10d). This is studied in more detail.
We can conclude that the screening resulted in an optimal
parameter array with all the investigated parameters set
high.

Table 1
Parameter settings of the screening phase

Preheating temperature (C)


Preheating time (s)
Mould pressure (bar)
Mould temperature (C)
Holding time (s)

Low

High

220
60
2.2
50
30

260
180
45
125
120

4.2.2.2. First optimisation. As the preheating temperature


is limited to the degradation temperature of the PP matrix
and the mould temperature should allow for a full
consolidation of the laminate, these two parameters could
not be further increased. Hence, only the preheating time,
mould pressure and holding time are raised during the next
optimisation step (Table 2) where the interaction between

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675

Fig. 8. Effect of the parameter settings on the flexural modulus of a split-warpknit laminate.

Fig. 9. Effect of the parameter settings on the bending strength of a split-warpknit laminate.

Fig. 10. (a) Interaction between the mould temperature and pressure on the flexural modulus. (b) Interaction between the mould temperature and pressure on
the flexural strength. (c) Interaction between the preheating temperature and time on the flexural modulus. (d) Interaction between the preheating time and
holding time on the flexural strength.

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Table 2
Parameter settings of the first optimisation step (preheating temperature
260C and mould temperature 125C)

Preheating time (s)


Mould pressure (bar)
Holding time (s)

Table 3
Settings for holding and preheating time during the second optimisation
step

Low

High

Holding time (s)

Preheating time (s)

180
45
180

240
60
240

160
140
120
100

276
312
348
384

the preheating time and the holding time was further


investigated. A full factorial design L8 is carried out.
Increasing the pressure further improves the bending
performance of the laminate (Fig. 11) due to better infiltration of the thermoplastic into the fibre bundles and hence
better efficiency of the reinforcement. It could also be seen
that at a low holding time, an increasing preheating time is
beneficial. When increasing the preheating time at high
preheating temperature, the viscosity of the thermoplastic
matrix decreases and small voids are easier filled with
matrix. The void volume is lower (decreases from 5.2 to
4%), resulting in a better mechanical performance. One
has, however, to be careful regarding degradation by oxidation of the PP matrix when preheated at too high a temperature for too long a time.
4.2.2.3. Second optimisation. Consequently, the pressure
is increased to the maximum allowed pressure of the press
(about 88 bar) and the interaction between the preheating
time and holding time is examined in more detail towards a
lower holding time (economically beneficial) and a higher
preheating time.
The parameter values are calculated in the direction of the
steepest slope of the plane of the measurements, obtained
during the former optimisation step (Table 3). Fig. 12
clearly shows the increase in bending strength for a lower
holding time and higher preheating time. Because the pressing cost mainly determines the production cost of the part, it
is economically favourable to work towards a low holding
time in the press (lower operating costs) and if necessary, a
longer preheating time. It is not clear, however, from this set
of experiments, which of the two parameters plays the
predominant role. This will be investigated in the third
optimisation step. A higher pressure gave no further
improvement. Though an increase in pressure indeed
enhances the ease of infiltration of the viscous polymer in
the closely packed fibre bundles, the fibre bundle is
squeezed together when too high a pressure is applied and

no further impregnation seems possible. It is also clear that


the applied pressure is much lower than the pressure applied
during the classical GMT process (150200 bars).
4.2.2.4. Third optimisation. A composite design method
of elliptical shape is applied to model the non-linear
interaction of the preheating and holding time on the
flexural behaviour. The settings, calculated to maintain an
elliptical shape, are given in Fig. 13. The pressure is set at an
optimum of 60 bar, because a further increase did not show
any improvement in the flexural behaviour. A quadratic
regression model is computed to model the response
surface for the flexural modulus and strength (Figs. 14 and
15). Though a further increase in the preheating time at
relatively low holding time leads to an improvement in
the bending performance, no more optimisation steps are
undertaken because a too long preheating time is
economically detrimental and increases the danger of
degradation of the polymer matrix.
After evaluation of the effects of the different parameters
and completing several optimisation steps, an optimal
processing window for the GMT cold pressing of splitwarpknit composite laminates is derived.
Preheating
preheating time: 540 s
preheating temperature: 260C
Cold pressing
mould temperature: 125C
mould pressure: 60 bar
holding time at pressure: 100 s

4.2.3. Validation of the optimal processing window


Because only flexural tests were carried out during the
optimisation so far, tensile tests on cross ply laminates

Fig. 11. The influence of pressure on the bending performance of a hybrid split-warpknit laminate.

S. Baeten, I. Verpoest / Composites: Part A 30 (1999) 667682

Fig. 12. The flexural strength as a function of holding and preheating time
for a hybrid split-warpknit laminate.

677

(90,0,90)2s were also carried out to validate the optimal


parameter set. The correlation between the tensile and bending modulus and strength is shown in Figs. 16 and 17 as a
function of processing parameters (see Table 4), showing a
quite linear relation. A comparison with the hot matched-die
moulding method is performed (point 9-CLASS).
At the optimal processing conditions, the mechanical
performance (tensile and bending behaviour) of the cold
pressed laminates almost reaches the quality of the inmould hot pressed laminates. Microscopy (see Figs. 18
20) yielded the presence of larger matrix rich regions and
a less even fibre distribution when compared to composites
produced by the classical matched-die moulding process.

Fig. 13. Elliptical parameter array for the composite design method.

Fig. 14. Modelled surface for the flexural modulus (composite design): interaction between preheating and holding time.

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Fig. 15. Modelled surface for the flexural strength (composite design): interaction between preheating and holding time.

This fact and the high void fraction of 5% (Table 5) can be


claimed to be responsible for the lower mechanical properties obtained with the adapted GMT process.
4.3. Evaluation of the impregnation quality
Optical transmission light microscopy visualises the
impregnation quality (i.e. presence of void areas) and the
fibre distribution throughout the composite.
In non-twisted split-film glass fibre yarns, the impregnation is mainly a two step process [9]:

intra-bundle impregnation
inter-bundle impregnation
After consolidation, the individual fibre bundles are still
visible despite the temperature and pressure. The higher the
impregnation pressure and the longer the time, the more
homogeneous the fibre distribution within the fibre bundle
will be [18,21,22]. The impregnation steps hence consist of
two main steps [22].
Initially separated fibre bundles are flattened out and
move towards each other when pressure is applied.

Fig. 16. Correlation between the tensile and flexural modulus for the split-warpknit laminates (see Table 4).

S. Baeten, I. Verpoest / Composites: Part A 30 (1999) 667682

679

Fig. 17. Correlation between the tensile and flexural strength for the split-warpknit laminates (see Table 4).

Table 4
Parameter set of the laminates, tested in tension
Type

Preheating time (s)

Preheating temperature (C)

Mould pressure (bar)

Mould temperature (C)

Holding time (s)

1-GMT
2-GMT
3-GMT
4-GMT
5-GMT
6-GMT
7-GMT
8-GMT
9-classical

180
180
180
240
180
180
380
610

260
220
220
260
260
260
260
260

2.2
45
45
60
45
45
60
60
20

50
50
125
125
125
125
125
125
240

30
30
120
180
120
120
100
70
300

Fig. 18. Non-homogeneous fibre distribution and matrix rich zones for a
non-optimal GMT cold pressing technique.

Fig. 19. More homogeneous fibre distribution for optimal GMT cold pressing cycle.

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Table 6
Cost comparison of the raw material for textile structures

Fig. 20. Uniform fibre distribution of matched-die moulded laminate.

This phase already starts during the conductive preheating where low pressure is applied to avoid the uncontrolled shrinkage of the PP ribbons. If the temperature
reaches the melt temperature of the thermoplastic matrix,
the polymer melts and tends to separate out of the
bundles to fill the spaces between them (inter-bundle
impregnation). The border of the reinforcing fibre is
clearly visible.
Consequently, the molten matrix infiltrate in the fibre
bundles and wet-out the individual fibres under the
applied pressure.
Because a cold pressing is applied during the GMT technique, the viscosity of the thermoplastic matrix decreases
very rapidly and a full melt-impregnation of the individual
fibres is hence not possible. The border of the fibre bundles
remains clear, resulting in a less homogeneous fibre distribution where matrix rich zones separate non-fully wetted
fibre bundles (Figs 18 and 19). Moreover, the non-meltable
stitches act as a periodic screen to the bulk flow of the
thermoplastic matrix between the fibre bundles. For this
reason, the fibre distribution is even for the optimal classical
matched-die moulding process not perfectly homogeneous
(Fig. 20).
Table 5
Comparison of the mechanical properties and void content for the GMT
cold pressed and the classical matched-die moulded laminates

Fibre volume fraction (%)


Matrix volume fraction (%)
Void fraction (%)
Flexural modulus (GPa)
Flexural strength (MPa)
Tensile modulus (GPa)
Tensile strength (MPa)

Matched-die
moulding

GMT cold
pressing

38.5
60.0
1.5
6.8
99.4
17.0
317.2

32.0
63.0
5.0
5.6
91.0
13.6
268.4

Material

Price index

Remarks

PP polymer
PP filaments
PP film

100
450
250

Granulates

Glass fibres
Twintex-PP/glass

200
280

Film split, stretched


and wound on bobbins
Co-mingled yarn

The presence of air bubbles or voids also results in poor


fibre wetting and consequently poor fibre bonding yielding
composite parts with non-uniform mechanical strength and
a rough surface quality [23]. This could be clearly noticed
during mechanical testing of the cold pressed composite
plates where, besides the high void fraction (Table 5) a
high standard deviation was also observed.
4.4. Economical comparison between GMT and splitwarpknit
The market for glass mat thermoplastic composites is
estimated to be around 15.000 tons/year (more than
37 MECU/year) [10]. The market share of the split-warpknits could become very substantial due to the fact that the
material has, compared to GMT, superior properties and a
competitive cost, and compared to thermosetting products
(SMC, BMC) better working conditions and a positive
impact on the environment (recycling). The material is
also cost-competitive compared to Twintex-based (Vetrotex) textile structures.
The sectors which seem to be most interesting for the
split-warpknit textiles are:
automotive;
electro/electronics;
civil engineering.
On the market, different thermoplastic textile structures
exist. In these existing technologies different methods are
used to combine the polymer with the reinforcing fibres, like
powder impregnated yarns (FIT-process), co-mingled yarns
(Destex, Twintex) and others. All these techniques are
expensive compared to split-warpknits. The reasons for
the cost-efficiency of the split-warpknits are situated on
three different levels.
Level 1: Cost of the raw material
All textile structures use almost the same reinforcing
fibres. The differences between the structures is especially the form in which the polymer is used. For the
split-warpknit a film is used as the base polymer
product. This film must have some special characteristics, but it can be produced with a very high efficiency,
for a low cost compared to polymer filaments. In Table
6, a comparison of the cost is presented.

S. Baeten, I. Verpoest / Composites: Part A 30 (1999) 667682

681

Table 7
Price estimation based on material cost of September 97 and bobbin technology for the split-warpknits
Material

Weight (g/m 2)

Width (cm)

Reinforcement

Vol.%

Cost (ECU/kg)

Split-warpknit
Twintex warpknit

673
700

130
130

Uni-axial
Uni-axial

52
50

4.2
6.7

Level 2: Cost of the split-film productioncombining


polymer and reinforcing fibres
In the split-warpknits, the polymer and the reinforcing
fibres are combined in the knitting step. This can be
done in three different ways:
Bobbins of glass fibres are used to warp on a beam,
placed in the knitting machine.
A FSSB (FolienSchneidStreck und Baumanlage) is
used to split, stretch and warp the beam in one operation.
With the ISO technique the film is split and oriented
and only tied into the guides of the knitting machine
when the product is started up for the first time.
Level 3: Production of the textile structure
Knitting is cost-efficient compared to weaving:
production speed of the knitting machine is independent of the width of the machine when only warp
knitting is used;
multi-axial and multi-layer textile structures can be
produced in one step;
non-wovens can be introduced into the structure.
Based on the Bobbin technology, the cost of the splitwarpknit structure is calculated (Table 7).
It can be concluded that split-warpknit textile structures
are cost-competitive with existing long fibre reinforced thermoplastic textile structures.
5. Conclusions
A new cost-effective thermoplastic textile preform,
containing both non-crimp reinforcing fibres and thermoplastic matrix ribbons, is made by weft-inserted multiaxial warp knitting. The final composite part is produced
by simple pressing the dry textile preform without any
further addition of matrix material. A thermoplastic PPmatrix/glass fibre system well suited to both split-warpknitting and composite production with short impregnation
times has been developed. It has been show that this new
split-warpknit is cost-competitive with existing long-fibre
reinforced thermoplastic textile structures.
An adapted GMT cold pressing technique, allowing for
the fast, one step production from dry textile preform to final
thermoplastic composite part, has been presented. After
evaluation of the different heating systems, only conductive
heating of the pile of dry textile layers between the platens
of a hot press at very low pressure (4 bar) is feasible to

prevent the thermoplastic ribbons from shrinking and


distorting the fibre architecture. During the preheating by
conduction, Teflon foil had to be used to prevent sticking of
the thermoplastic matrix to the heating device.
The Taguchi experimental design method has been
successfully applied to further optimise the GMT cold
pressing method to produce split-warpknit thermoplastic
composites. The influence of the processing parameters
preheating temperature and time, mould pressure and
temperature, and holding time at pressureon the bending
performance of the final laminates has been evaluated. An
optimal processing window is determined.
While it was shown that the GMT cold pressing technique
is feasible for split-warpknits, it still yields somewhat lower
composite mechanical properties compared to the hot
matched-die pressing process. Nevertheless, it can be very
worthwhile to consider it in low-cost applications, especially because existing equipment can be used.

Acknowledgements
This research is suppported by the European Community
Research Programme Brite-Euram, Project no BE7256-93,
Contract number BRE2-CT94-0552. The authors gratefully
acknowledge the financial contribution by the commission
and the contribution of the different partners, especially
Prof. K. Schulte (TUHamburg-Harburg, Germany), Walter
Zah (Karl Mayer, Germany), Dr Edith Mader (Institut fur
Polymerforschung, Germany), Carl-Hakan Andersson
(Lund University, Sweden), Kjell Eng (Engtex, Sweden).
Part of this research has been financed with a specialisation
grant of the Flemish Institute for the Promotion of Scientific
and Technological Research in Industry (IWT). This text
presents research results of the Belgian programme on Interuniversity Poles of Attraction initiated by the Belgian State,
Prime Ministers Office, Science Policy Programming. The
scientific responsibility is assumed by its authors.

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